A colorable pigment was prepared by dye adsorption onto titanium dioxide and subsequent silane coating. The effects of pH value, dye concentration, and adsorption times on dye adsorption were discussed. Large adsorption capacity of an anionic dye was obtained at pH value of 2 and the adsorption process was well described by the Langmuir isotherm model. Good dyeability and color fastness of pigment dyed fabric were achieved in the normal life cycle under sunlight. The decoloration of pigment was realized through photocatalytic degradation of dye molecules by titanium dioxide under ultraviolet irradiation when reusing the pigment dyed textiles after disposal. The new absorption peaks in the FTIR spectrum at 2924.95 cm-1, 1714.91 cm-1, 1461.17 cm-1, and 1289 cm-1 verified silane modification. Silane modification improved fixation of dyes onto the pigment and immobilization of pigments onto substrates. The close attachment of silane coating layer to titanium dioxide was conducive to photodegradation of dye molecules in the pigment.